The possibility of influencing resonance energy transfer through the input of off-resonant pulses of laser radiation is the subject of recent research. Attention is now focused on systems in which resonance energy transfer is designedly precluded by geometric configuration. Here, through an optically nonlinear mechanism - optically controlled resonance energy transfer - the throughput of non-resonant pulses can facilitate energy transfer that is, in their absence, completely forbidden. The system thus functions as an optical buffer, with excitation throughput switched on by the secondary beam. For applications, a system based on two parallel nano-arrays is envisaged. This paper will establish and discuss the principles - those that can be exploited to enhance switching characteristics and efficiency, and others (such as off-axis excitation transfer) that may represent cross-talk limitations. Principles to be explored in detail are the interplay between geometric features, including the array architecture and repeat distance (lattice constant), the array spacing and translational symmetry, the orientations of the transition dipoles, and the magnitude of the relevant components of the nonlinear response tensors. The aim is, through a determination of key parameters, to inform a program of optimization that can deliver specific criteria for realizing the most efficient systems for implementation.
The possibility of influencing resonance energy transfer through the input of off-resonant pulses of laser radiation is the subject of recent research. Attention is now focused on systems in which resonance energy transfer is designedly precluded by geometric configuration. Here, through an optically nonlinear mechanism - optically controlled resonance energy transfer - the throughput of non-resonant pulses can facilitate energy transfer that is, in their absence, completely forbidden. The system thus functions as an optical buffer, with excitation throughput switched on by the secondary beam. For applications, a system based on two parallel nano-arrays is envisaged. This paper will establish and discuss the principles - those that can be exploited to enhance switching characteristics and efficiency, and others (such as off-axis excitation transfer) that may represent cross-talk limitations. Principles to be explored in detail are the interplay between geometric features, including the array architecture and repeat distance (lattice constant), the array spacing and translational symmetry, the orientations of the transition dipoles, and the magnitude of the relevant components of the nonlinear response tensors. The aim is, through a determination of key parameters, to inform a program of optimization that can deliver specific criteria for realizing the most efficient systems for implementation.
Resonance energy transfer (RET) is a near-field mechanism for propagating optical energy between particles with suitably matching frequency response. The process communicates electronic excitation between suitably disposed (donor and acceptor) dipoles in close proximity, activated on excitation of the donor. In a multi-component system the transfer of excitation between any given donor and acceptor is usually passive, and it competes with loss mechanisms such as radiative decay and the possibility of transfer to one or more other acceptors. It thus appears that any potential exploitation of RET for optical switching is compromised by the innate passivity of the process. Now it emerges that there is a direct, all-optical route to introduce the necessary control. In a system constructed to satisfy frequency-matching conditions, but designedly to inhibit RET by geometric configuration, the throughput of laser pulses can facilitate energy transfer processes that would otherwise be forbidden, by laser-assisted resonant energy transfer. Suitably configuring an arrangement of transition dipoles, it proves possible to design parallel planar arrays of optical donor and acceptor particles such that the transfer of energy from any single donor, to its counterpart in the opposing plane, can be switched by appropriate laser radiation. As the energy transfer is itself mediated electromagnetically, the device operates as an optical transistor. For simplicity, a pair of two-dimensional arrays is envisaged, each consisting of equally spaced, identical particles arranged on a square lattice. A detailed appraisal of the system, including a consideration of competing processes, suggests that this configuration offers a new basis for the design of optically activated nanoscale transistor arrays.
In a molecular system of energy donors and acceptors, resonance energy transfer is the primary mechanism by means of which electronic energy is redistributed between molecules, following the excitation of a donor. Given a suitable geometric configuration it is possible to completely inhibit this energy transfer in such a way that it can only be activated by application of an off-resonant laser beam: this is the principle of optically controlled resonance energy transfer, the basis for an all-optical switch. This paper begins with an investigation of optically controlled energy transfer between a single donor and acceptor molecule, identifying the symmetry and structural constraints and analyzing in detail the dependence on molecular energy level positioning. Spatially correlated donor and acceptor arrays with linear, square, and hexagonally structured arrangements are then assessed as potential configurations for all-optical switching. Built on quantum electrodynamical principles the concept of transfer fidelity, a parameter quantifying the efficiency of energy transportation, is introduced and defined. Results are explored by employing numerical simulations and graphical analysis. Finally, a discussion focuses on the advantages of such energy transfer based processes over all-optical switching of other proposed forms.
By suitably configuring an arrangement of transition dipoles, it proves possible to design parallel planar arrays of optical donor and acceptor particles such that the transfer of energy from any single donor, to its counterpart in the opposing plane, can be switched by throughput laser radiation of an appropriate intensity, frequency and polarization. As the resonance energy transfer is itself mediated electromagnetically, the device operates as an optical transistor based on laser-assisted energy transfer.
Through photonic mechanisms based on near-field coupling, laser radiation can engage with resonant energy transfer in a variety of suitably designed materials and molecular structures. Energy that has been acquired, through the initial absorption of resonant laser light, undergoes transfer between chromophores only on the throughput of off-resonant light, the process known as laser-assisted resonance energy transfer. The comprehensive results that are presented here extend and generalize the theory for both single and dual beam configurations, producing results that are applicable to media of various types including doped crystals, heterogeneous multichromophore solids, and solutions. The detailed principles, here explained in terms of both energetics and optical selection rule criteria, are specifically illustrated for a variety of materials. It is shown how general application of the theory can facilitate the elucidation of experiments, by clearly interpreting the effects of laser polarization manipulation. On further analysis of the photophysical mechanisms it is also demonstrated that such effects represent an entirely practicable basis for optical switching and logic gate operation. The additional polarization selectivity afforded by a two-beam setup proves to allow the most complete system control. With such a configuration, there is considerable promise for the realization of new optically driven logic and molecular devices.
The theory of non-resonant optical processes with intrinsic optical nonlinearity, such as harmonic generation, has been widely understood since the advent of the laser. In general, such effects involve multiphoton interactions that change the population of each input optical mode or modes. However, nonlinear effects can also arise through the input of an off-resonant laser beam that itself emerges unchanged. Many such effects have been largely overlooked. Using a quantum electrodynamical framework, this review provides detail on such optically nonlinear mechanisms that allow for a controlled increase or decrease in the intensity of linear absorption and fluorescence and in the efficiency of resonance energy transfer. The rate modifications responsible for these effects were achieved by the simultaneous application of an off-resonant beam with a moderate intensity, acting in a sense as an optical catalyst, conferring a new dimension of optical nonlinearity upon photoactive materials. It is shown that, in certain configurations, these mechanisms provide the basis for all-optical switching, i.e., the control of light-by-light, including an optical transistor scheme. The conclusion outlines other recently proposed all-optical switching systems.
It is shown that, in the optical near field, the interaction of two polarized laser beams with different frequencies can promote a transfer of energy between suitably placed donor and acceptor particles, through a process that is rigorously forbidden in the absence of the laser light. The mechanism, which operates through stimulated Raman scattering by the donor-acceptor pair, is identified and characterized by quantum electrodynamical calculation. The results suggest efficiency levels comparable to conventional resonance energy transfer. Optical switching applications are envisaged.